FACULTY OF ENGINEERING AND ARCHITECTURE

Department of Chemical Engineering and Technical Chemistry Laboratory for Chemical Technology Director : Prof. Dr. Ir. Guy B. Marin

Short contact time catalytic partial oxidation of natural gas

Aim Acquiring a detailed understanding of the reaction mechanism in methane partial oxidation. Determination of the most suited reactor configuration for industrial implementation. Justification The economic exploitation of stranded natural gas or biogas constitutes a gigantic potential to serve the worlds greed for liquid fuels and chemicals. The latter can be obtained from it via synthesis gas, i.e. CO/H2 mixtures. Steam reforming of methane, a highly endothermic reaction, is the most commonly applied process for synthesis gas production. Partial oxidation of methane with dioxygen, however, is a promising alternative that is exothermic and yields synthesis gas with an optimal H2 to CO ratio for further processing via, e.g., Fischer-Tropsch synthesis. Catalytic partial oxidation (CPO) at millisecond contact times allows in principle an optimal temperature control and, hence, the most economical conversion of bio to synthesis gas. Such short contact times can be established in a novel reactor technology: a rotary fluid bed with static reactor geometry also called Gas-Solid Vortex Reactor (GSVR). In this technology the centrifugal rather than the gravitational force maintains the catalyst in the reactor while being fluidized allowing high gas velocities without excessive pressure drop. Program In order to assess the potential of the rotary fluid bed technology for methane partial oxidation, several parallel and consecutive activities will be deployed: Literature survey on the detailed reaction mechanism of methane partial oxidation. Analysis of evidence for the direct versus the indirect mechanism will be performed and will form the basis of the decision whether additional experimental investigations will be required or not. Only the direct mechanism allows the better temperature control. (micro)Kinetic model construction: An adequate kinetic model is a conditio sine qua non for a proper assessment of laboratory and industrial reactor behaviour via simulation. The challenge will be to establish the optimal combination of reactor and reaction model. In this respect (micro)kinetic models of different complexity will be constructed that will be implemented in reactor models containing various degrees of detail. Particular attention will be given to the introduction of so-called catalyst descriptors in the microkinetic models. The latter will allow to simulate the effect of catalyst properties on product selectivities. The possible interaction between heterogeneously catalysed steps and non-catalytic gas phase reactions will be given attention. Reactor simulations: reactor models accounting for the transport phenomena occurring on the scale of the catalyst pellet as well as those occurring on the scale of the reactor will be implemented in available Computational Fluid Dynamics (CFD) codes. The latter will be applied to assess the feasibility of the GSVR for CPO as well to determine the optimal industrial process conditions. Advisors: Joris W. Thybaut and Guy B. Marin Funding: Advanced Grant of the European Research Council
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